Acquiring hybrid molecular crystal materials through high-throughput screening†

As a class of inorganic van der Waals (vdW) molecular crystal materials, α-phase Sb₂O₃ (hereafter referred to as Sb₂O₃) has demonstrated promising potential in the field of dielectric materials due to its high dielectric constant, excellent room-temperature stability, and favorable processing compatibility with two-dimensional (2D) semiconductors. However, its relatively narrow bandgap (compared to conventional dielectric materials) has constrained its implementation in 2D semiconductor devices. To overcome this limitation, we developed a novel approach leveraging synergistic effects through the hybridization of distinct molecular crystals—specifically Sb₂O₃ and As₂O₃. Employing high-throughput screening via structure prediction software, followed by comprehensive stability analyses, we successfully identified a stable hybrid inorganic vdW molecular crystal with the space group F3m. Our characterization revealed that this hybrid material exhibits exceptional mechanical flexibility alongside superior dielectric properties, achieving a high-k dielectric constant exceeding 8 and an impressive direct bandgap of 4.55 eV. These results demonstrate successful property modulation through the strategic hybridization of molecular cages. The significance of these findings extends beyond immediate applications, advancing our fundamental understanding of dielectric behavior in hybrid molecular crystals while establishing new pathways for designing vdW inorganic molecular crystals. This work provides a robust theoretical framework for future experimental studies in this field.